Dynamical reconstruction of the exciton in LiF with inelastic x-ray scattering.

Proceedings of the National Academy of Sciences of the United States of America
Peter AbbamonteWei Ku

Abstract

The absorption of light by materials proceeds through the formation of excitons, which are states in which an excited electron is bound to the valence hole it vacated. Understanding the structure and dynamics of excitons is important, for example, for developing technologies for light-emitting diodes or solar energy conversion. However, there has never been an experimental means to study the time-dependent structure of excitons directly. Here, we use causality-inverted inelastic x-ray scattering (IXS) to image the charge-transfer exciton in the prototype insulator LiF, with resolutions Delta t = 20.67 as (2.067 x 10(-17) s) in time and Delta x = 0.533 A (5.33 x 10(-11) m) in space. Our results show that the exciton has a modulated internal structure and is coherently delocalized over two unit cells of the LiF crystal (approximately 8 A). This structure changes only modestly during the course of its life, which establishes it unambiguously as a Frenkel exciton and thus amenable to a simplified theoretical description. Our results resolve an old controversy about excitons in the alkali halides and demonstrate the utility of IXS for imaging attosecond electron dynamics in condensed matter.

References

Oct 6, 2000·Physical Review Letters·W A CaliebeK Hamalainen
Oct 26, 2002·Physical Review Letters·Wei KuR T Scalettar
Jul 13, 2004·Physical Review Letters·P AbbamonteS M Gruner
Sep 2, 2006·Nature Materials·Gregory D Scholes, Garry Rumbles

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Citations

Dec 19, 2012·Annual Review of Physical Chemistry·Shaul MukamelJason D Biggs
Jun 8, 2015·The Journal of Chemical Physics·R WebsterN M Harrison
Oct 21, 2009·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Robert H CoridanGerard C L Wong
Apr 20, 2010·Advanced Materials·Peter AbbamonteDiego Casa
Feb 27, 2016·Physical Review Letters·Pierluigi CudazzoMatteo Gatti
Mar 4, 2011·Optics Express·Hatem DachraouiUlrich Heinzmann
Mar 5, 2015·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Pierluigi CudazzoMatteo Gatti
Nov 21, 2015·Physical Review Letters·Ryky NelsonWei Ku
Mar 17, 2011·Physical Review Letters·J LienemannH Winter
Mar 17, 2011·Physical Review Letters·T T FisterP A Salvador
Sep 28, 2010·Physical Review Letters·Matteo GattiAngel Rubio
Apr 1, 2020·Journal of Chemical Theory and Computation·Xiao Wang, Timothy C Berkelbach

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